Electronegative Phosphorus-Integrated Co2+ Active Sites for Enhanced Electrocatalytic Nitrogen Reduction DOI

Yuanyuan Xiong,

Jingxian Li, Xiaoxuan Wang

et al.

Inorganic Chemistry, Journal Year: 2024, Volume and Issue: 63(17), P. 7886 - 7895

Published: April 15, 2024

In the quest for proficient electrocatalysts ammonia's electrocatalytic nitrogen reduction, cobalt oxides, endowed with a rich d-electron reservoir, have emerged as frontrunners. Despite previously evidenced prowess of CoO in this realm, its ammonia yield witnesses pronounced decline reaction unfolds, phenomenon linked to electron attrition from Co2+ active sites during reduction (ENRR). To counteract vulnerability, we harnessed electron-laden phosphorus (P) elements dopants, aiming recalibrate electronic equilibrium pivotal Co site, thereby bolstering both catalytic performance and stability. Our empirical endeavors showcased doped P-CoO's superior credentials: it delivered an impressive 49.6 and, notably, Faradaic efficiency (FE) 9.6% at −0.2 V versus RHE, markedly eclipsing undoped counterpart. Probing deeper, suite ex-situ techniques, complemented by rigorous theoretical evaluations, was deployed. This dual-pronged analysis unequivocally revealed CoO's propensity electron-driven valence metamorphosis Co3+ post-ENRR. stark contrast, P-CoO, fortified P doping, exhibits discernibly augmented yield. Crucially, P's intrinsic ability staunch leakage locus ENRR ensures preservation state, culminating enhanced dynamism fortitude. investigation not only illuminates intricacies site modulation but also charts navigational beacon further enhancements domain.

Language: Английский

Advances in modification of Bi2MoO6 and its photocatalysis: A review DOI
Mingjie Lyu, Changmin Wang,

Youzhuang Rong

et al.

Journal of Alloys and Compounds, Journal Year: 2024, Volume and Issue: 982, P. 173759 - 173759

Published: Feb. 3, 2024

Language: Английский

Citations

24
Multivalent Sulfur Vacancy‐Rich NiCo2S4@MnO2 Urchin‐Like Heterostructures for Ambient Electrochemical N2 Reduction to NH3 DOI
Muhammad Asim Mushtaq, Anuj Kumar, Ghulam Yasin

et al.

Small, Journal Year: 2024, Volume and Issue: 20(31)

Published: March 5, 2024

Abstract Innovative advances in the exploitation of effective electrocatalytic materials for reduction nitrogen (N 2 ) to ammonia (NH 3 are highly required sustainable production fertilizers and zero‐carbon emission fuel. In order achieve footprints renewable NH production, electrochemical N reaction (NRR) provides a favorable energy‐saving alternative but it requires more active, efficient, selective catalysts. current work, sulfur vacancy (Sv)‐rich NiCo S 4 @MnO heterostructures efficaciously fabricated via facile hydrothermal approach followed by heat treatment. The urchin‐like Sv‐NiCo serve as cathodes, which demonstrate an optimal yield 57.31 µg h −1 mg cat Faradaic efficiency 20.55% at −0.2 V versus reversible hydrogen electrode (RHE) basic electrolyte owing synergistic interactions between MnO . Density functional theory (DFT) simulation further verifies that Co‐sites beneficial lowering energy threshold adsorption successive protonation. Distinctive micro/nano‐architectures exhibit high NRR activities might motivate researchers explore concentrate on development ambient generation.

Language: Английский

Citations

24
Defect-rich AuCu@Ag nanowires with exclusive strain effect accelerate nitrate reduction to ammonia DOI

Songliang Liu,

W.F. Miao,

Kun Ma

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 350, P. 123919 - 123919

Published: April 24, 2024

Language: Английский

Citations

18
Enhancing Green Ammonia Electrosynthesis Through Tuning Sn Vacancies in Sn-Based MXene/MAX Hybrids DOI Creative Commons
Xinyu Dai, Zhenyi Du, Ying Sun

et al.

Nano-Micro Letters, Journal Year: 2024, Volume and Issue: 16(1)

Published: Jan. 16, 2024

Abstract Renewable energy driven N 2 electroreduction with air as nitrogen source holds great promise for realizing scalable green ammonia production. However, relevant out-lab research is still in its infancy. Herein, a novel Sn-based MXene/MAX hybrid abundant Sn vacancies, Sn@Ti CT X /Ti SnC–V, was synthesized by controlled etching SnC MAX phase and demonstrated an efficient electrocatalyst electrocatalytic reduction. Due to the synergistic effect of heterostructure, existence vacancies highly dispersed active sites, obtained SnC–V exhibits optimal NH 3 yield 28.4 µg h −1 mg cat excellent FE 15.57% at − 0.4 V versus reversible hydrogen electrode 0.1 M Na SO 4 , well ultra-long durability. Noticeably, this catalyst represents satisfactory rate 10.53 home-made simulation device, where commercial electrochemical photovoltaic cell employed power source, ultrapure water feed stock. The as-proposed strategy potential toward production terms financial cost according systematic technical economic analysis. This work significance large-scale

Language: Английский

Citations

16
A High-Throughput Screening toward Efficient Nitrogen Fixation: Transition Metal Single-Atom Catalysts Anchored on an Emerging π–π Conjugated Graphitic Carbon Nitride (g-C10N3) Substrate with Dirac Dispersion DOI
Qiang Zhang, Xian Wang, Fuchun Zhang

et al.

ACS Applied Materials & Interfaces, Journal Year: 2023, Volume and Issue: 15(9), P. 11812 - 11826

Published: Feb. 21, 2023

TM-Nx is becoming a comforting catalytic center for sustainable and green ammonia synthesis under ambient conditions, resulting in increasing interest single-atom catalysts (SACs) the electrochemical nitrogen reduction reaction (NRR). However, given poor activity unsatisfactory selectivity of existing catalysts, it remains long-standing challenge to design efficient fixation. Currently, two-dimensional (2D) graphitic carbon-nitride substrate provides abundant evenly distributed holes stably supporting transition-metal atoms, which presents fascinating prospect overcoming this promoting NRR. An emerging holey skeleton with C10N3 stoichiometric ratio (g-C10N3) from supercell graphene constructed, outstanding electric conductivity achieving high-efficiency NRR due Dirac band dispersion. Herein, high-throughput first-principles calculation carried out evaluate feasibility π-d conjugated SACs single TM atom anchored on g-C10N3 (TM = Sc-Au) We find that W metal embedded (W@g-C10N3) can compromise ability adsorb key target species (N2H NH2), hence acquiring an optimal behavior among 27 TM-candidates. Our calculations demonstrate W@g-C10N3 shows well-suppressed HER and, impressively, low energy cost -0.46 V. Additionally, all-around descriptors are proposed uncover fundamental mechanism activity, 3D volcano plot (limiting potential, screening strategy, electron origin) uncovers trend, quick prescreening numerous candidates. Overall, strategy structure- activity-based TM-Nx-containing unit will offer useful insight further theoretical experimental attempts.

Language: Английский

Citations

38
Strategies to achieve effective nitrogen activation DOI Creative Commons
Bin Chang, Huabin Zhang, Shuhui Sun

et al.

Carbon Energy, Journal Year: 2024, Volume and Issue: 6(5)

Published: Feb. 23, 2024

Abstract Ammonia serves as a crucial chemical raw material and hydrogen energy carrier. Aqueous electrocatalytic nitrogen reduction reaction (NRR), powered by renewable energy, has attracted tremendous interest during the past few years. Although some achievements have been revealed in aqueous NRR, significant challenges also identified. The activity selectivity are fundamentally limited activation competitive evolution. This review focuses on hurdles of delves into complementary strategies, including materials design system optimization (reactor, electrolyte, mediator). Then, it introduces advanced interdisciplinary technologies that recently emerged for using high‐energy physics such plasma triboelectrification. With better understanding corresponding mechanisms coming years, these potential to be extended further applications. provides insight stability different systems. We then recommend rigorous detailed protocol investigating NRR performance highlight several research directions this exciting field, coupling with applications, situ/operando characterizations, theoretical calculations.

Language: Английский

Citations

15
Enhanced N2 Adsorption and Activation by Combining Re Clusters and In Vacancies as Dual Sites for Efficient and Selective Electrochemical NH3 Synthesis DOI
Shaoquan Li, Yi‐Tao Liu, Yong‐Chao Zhang

et al.

Nano Letters, Journal Year: 2024, Volume and Issue: 24(2), P. 748 - 756

Published: Jan. 3, 2024

The electrochemical N2 reduction reaction (NRR) is a green and energy-saving sustainable technology for NH3 production. However, high activity selectivity can hardly be achieved in the same catalyst, which severely restricts development of NRR. In2Se3 with partially occupied p-orbitals suppress H2 evolution (HER), shows excellent presence VIn simultaneously provide active sites confine Re clusters through strong charge transfer. Additionally, well-isolated stabilized on by confinement effect result Re-VIn maximum availability. By combining as dual spontaneous adsorption activation, NRR performance enhanced significantly. As result, Re-In2Se3-VIn/CC catalyst delivers yield rate (26.63 μg h–1 cm–2) FEs (30.8%) at −0.5 V vs RHE.

Language: Английский

Citations

12
Unveiling cutting-edge progress in the fundamentals of MXene: Synthesis strategies, energy and bio-environmental applications DOI

Ikhtiar Gul,

Murtaza Sayed,

Tooba Saeed

et al.

Coordination Chemistry Reviews, Journal Year: 2024, Volume and Issue: 511, P. 215870 - 215870

Published: April 21, 2024

Language: Английский

Citations

12
Introduction of element Bi in the P-block promotes N2 activation for efficient electrocatalytic nitrogen reduction to produce ammonia DOI
Xiaoyue Chen,

Guangmin Ren,

Yaru Wang

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 355, P. 124173 - 124173

Published: May 10, 2024

Language: Английский

Citations

12
Bismuth-doped manganese molybdenum bimetallic oxide nanorods as a highly efficient nitrogen reduction catalyst DOI

Huhu Yin,

Ziyang Song, Xiujing Xing

et al.

Materials Chemistry Frontiers, Journal Year: 2024, Volume and Issue: 8(20), P. 3373 - 3382

Published: Jan. 1, 2024

Bi-doped MnMoO 4 nanorods prepared by a simple hydrothermal method exhibit an excellent electrocatalytic nitrogen gas reduction performance at −0.40 V vs. RHE.

Language: Английский

Citations

6